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• Nano-deposits at different deposition temperatures have hexagonal wurtzite structures with (1 0 1) plane. • Deposits prepared at 723 K have higher crystallinity with few dislocations' density. • Films deposited at 723 K demonstrate enhanced electrical properties. • Photoluminescence studies indicate near-white light emission across all thin films. • The total nonlinear susceptibility decreases as the deposition temperature rises. This study reports the influence of deposition temperature (573 K-773 K) on the microstructural, linear and nonlinear optical properties of zinc oxide nano thin films synthesized using the chemical spray pyrolysis method. Synthesized films are polycrystalline, exhibiting a dominant (1 0 1) orientation, for which the crystallite size is found to increase with deposition temperature up to 723 K followed by a decrease. Concurrently, the deposit prepared at 723 K showed improved electrical properties, i.e. higher charge carrier concentration and mobility. Optical studies reveal increased transmittance in the visible region and a gradual increase of optical bandgap with deposition temperature. The photoluminescence studies show a near-white light emission for all thin films, however, the density of defect states was comparatively higher for thin films deposited at lower temperatures. A saturable absorption behaviour was observed due to the presence of defects. The thin films show a negative refractive index with self-defocusing phenomena. The total nonlinear susceptibility is found to decrease with increasing deposition temperature, and the solution-processed functional thin films thus have potential implications for nonlinear optical applications such as nonlinear optical switching, optical memory management, and saturable absorbers. [ABSTRACT FROM AUTHOR]